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1.
J Colloid Interface Sci ; 665: 286-298, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38531274

ABSTRACT

Tailoring porous host materials, as an effective strategy for storing sulfur and restraining the shuttling of soluble polysulfides in electrolyte, is crucial in the design of high-performance lithium-sulfur (Li-S) batteries. However, for the widely studied conductive hosts such as mesoporous carbon, how the aspect ratio affects the confining ability to polysulfides, ion diffusion as well as the performances of Li-S batteries has been rarely studied. Herein, ordered mesoporous carbon (OMC) is chosen as a proof-of-concept prototype of sulfur host, and its aspect ratio is tuned from over âˆ¼ 2 down to below âˆ¼ 1.2 by using ordered mesoporous silica hard templates with variable length/width scales. The correlation between the aspect ratio of OMCs and the electrochemical performances of the corresponding sulfur-carbon cathodes are systematically studied with combined electrochemical measurements and microscopic characterizations. Moreover, the evolution of sulfur species in OMCs at different discharge states is scrutinized by small-angle X-ray scattering. This study gives insight into the aspect ratio effects of mesoporous host on battery performances of sulfur cathodes, providing guidelines for designing porous host materials for high-energy sulfur cathodes.

2.
ACS Macro Lett ; 12(8): 1071-1078, 2023 Aug 15.
Article in English | MEDLINE | ID: mdl-37462370

ABSTRACT

Despite the ever more versatile polymerization techniques that are becoming available, the synthesis of macromolecules with tailored functionalities can remain a lengthy endeavor. This becomes more conspicuous when the implementation of incompatible chemistries (i.e., strong polyelectrolytes) within sequence-controlled polymers is desired, often requiring (i) polymerization, (ii) chain extension, and (iii) postpolymerization modification. Herein, we explore the production of strong anionic/charge-neutral block copolymers (BCPs) in a one-pot fashion. This straightforward three-step process includes the synthesis of a macroinitiator and chain extension via rapid and efficient photomediated atom transfer radical polymerization, followed by in situ deprotection to expose the polyanionic domains. The resulting BCPs, which are strong amphiphiles by nature, are capable of self-assembly in aqueous media, as evidenced by dynamic light scattering, small-angle X-ray scattering, ζ-potential measurements, and transmission electron microscopy. We further demonstrate the versatility of our methodology by producing several BCPs through sampling of a single reaction mixture, enabling the straightforward production of strong polymer amphiphiles.

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